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Valence and Local Environment of Molybdenum in Aluminophosphate Glasses for Immobilization of High Level Waste from Uranium-Graphite Reactor Spent Nuclear Fuel Reprocessing

Published online by Cambridge University Press:  19 March 2015

Sergey V. Stefanovsky ,
Andrey A Shiryaev ,
Michael B. Remizov ,
Elena A. Belanova ,
Pavel A. Kozlov  and
Boris F. Myasoedov
Sergey V. Stefanovsky
Affiliation:
Frumkin Institute of Physical Chemistry and Electrochemistry RAS, Leninskii av. 31, Bld. 4, Moscow, 119071 Russia.
Andrey A Shiryaev
Affiliation:
Frumkin Institute of Physical Chemistry and Electrochemistry RAS, Leninskii av. 31, Bld. 4, Moscow, 119071 Russia.
Michael B. Remizov
Affiliation:
FSUE Production Association “Mayak”, Lenin st. 13, Ozersk Chelyabinsk reg. 456780 Russia
Elena A. Belanova
Affiliation:
FSUE Production Association “Mayak”, Lenin st. 13, Ozersk Chelyabinsk reg. 456780 Russia
Pavel A. Kozlov
Affiliation:
FSUE Production Association “Mayak”, Lenin st. 13, Ozersk Chelyabinsk reg. 456780 Russia
Boris F. Myasoedov
Affiliation:
Vernadsky Institute of Geochemistry and Analytical Chemistry RAS, Kosygin st. 19, Moscow 119071 Russia
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Abstract

Two Mo-bearing glasses considered as candidate forms for high level waste (HLW) a uranium-graphite reactor spent nuclear fuel (SNF) reprocessing were characterized. Incorporation of Mo in sodium aluminophosphate (SAP) glass increases its tendency to devitrification with segregation of orthophosphate phases. Valence state and local environment of Mo in the materials containing ∼2 wt.% MoO3 were determined by X-ray absorption fine structure (XAFS) spectroscopy. In the quenched samples composed of major vitreous and minor AlPO4 nearly all Mo is located in the vitreous phase as [Mo6+О6] units whereas in the annealed samples Mo is partitioned among vitreous and one or two orthophosphate crystalline phases in favor of the vitreous phase. Mo predominantly exists in a hexavalent state in distorted octahedral environment. Four oxygen ions are positioned at a distance of ∼1.71-1.73 Å and two - at a distance of 2.02-2.04 Å. Minor Mo(V) is also present as indicated by a response in EPR spectra with g ≈ 1.911-1.915.

Keywords

Moelectron spin resonanceextended x-ray absorption fine structure(EXAFS)
Type
Articles
Information
MRS Online Proceedings Library (OPL) , Volume 1744: Symposium EE – Scientific Basis for Nuclear Waste Management XXXVIII , 2015 , pp. 73 - 78
Copyright
Copyright © Materials Research Society 2015 

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